CN105144845A - Method for forming pattern of organic electroluminescent element - Google Patents
Method for forming pattern of organic electroluminescent element Download PDFInfo
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- CN105144845A CN105144845A CN201480022806.9A CN201480022806A CN105144845A CN 105144845 A CN105144845 A CN 105144845A CN 201480022806 A CN201480022806 A CN 201480022806A CN 105144845 A CN105144845 A CN 105144845A
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Classifications
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/20—Changing the shape of the active layer in the devices, e.g. patterning
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/70—Testing, e.g. accelerated lifetime tests
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/20—Changing the shape of the active layer in the devices, e.g. patterning
- H10K71/211—Changing the shape of the active layer in the devices, e.g. patterning by selective transformation of an existing layer
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/10—Apparatus or processes specially adapted to the manufacture of electroluminescent light sources
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
- H10K50/125—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light
- H10K50/13—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light comprising stacked EL layers within one EL unit
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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- Electroluminescent Light Sources (AREA)
Abstract
The objective of the present invention is to provide a method for forming a pattern of an organic electroluminescent element, which is capable of accurately forming a light emitting pattern having a desired luminance gradation. This method for forming a pattern of an organic electroluminescent element is a method for forming a light emitting pattern by irradiating an organic electroluminescent element, which is provided with an organic functional layer between a pair of electrodes, with light. This method for forming a pattern of an organic electroluminescent element is characterized in that the light emitting pattern is formed by controlling the light intensity and/or the irradiation time as a variation factor on the basis of the reciprocity failure characteristics with respect to the functional changes of the organic functional layer due to light irradiation.
Description
Technical field
The present invention relates to the pattern formation method of organic electroluminescent device.Particularly relate to the pattern formation method that correctly can form the organic electroluminescent device of the luminous pattern of the grade of the luminosity with expectation.
Background technology
Now, organic illuminating element receives publicity as slim luminescent material.
With regard to the organic illuminating element (hereinafter also referred to " organic EL element ") that make use of the electroluminescence (electroluminescence:EL) of organic material, for the complete solid-state components of film-type that can be luminous under the low-voltage of several V ~ tens of about V, there is the feature of high brightness, high-luminous-efficiency, the many excellences that slim, light weight is such.Therefore, the planar luminous body as the display panel, lighting source etc. of the backlight, label, emergency light etc. of various display receives publicity in recent years.
Such organic EL element is between pair of electrodes, be configured with the formation of organic function layer at least containing luminescent layer, the luminous light transmission electrode created in luminescent layer and be fetched to outside.Therefore, at least one in pair of electrodes is formed with the form of transparency electrode, takes out luminous light from transparency electrode side.In addition, organic EL element can obtain high brightness with low electric power, observability, response speed, the life-span, power consumption in excellent.
At this, motion has following method: in such organic EL element, adjust exposure while irradiate light relative to organic function layer in each regulation region, make the changes of function of organic function layer thus in each regulation region, form the luminous pattern of the grade of the luminosity with its variable quantity corresponding (such as with reference to patent documentation 1.)。In the method, to increase along with the long-pending accumulated light as ultraviolet intensity and irradiation time, the variable quantity of the function of organic function layer is also increased to prerequisite without exception and carries out Ultraviolet radiation.
But, the discoveries such as the present inventor: when being radiated at organic EL element by light and forming luminous pattern, with regard to the variable quantity of the function of organic function layer, even if irradiate the accumulated light [Ws/cm of the light in organic EL element
2] be certain, at the intensity [W/cm of light
2] different with the relation of irradiation time [s] time, the variable quantity of the function of organic function layer is also different.
Therefore, if be only conceived to accumulated light to carry out illumination to organic EL element, then according to the intensity of this light and the relation of irradiation time, the luminous pattern of the grade of the luminosity with expectation cannot sometimes be formed.
Prior art document
Patent documentation
Patent documentation 1: Japanese Unexamined Patent Publication 2012-28335 publication
Summary of the invention
The problem that invention will solve
The present invention completes in order to the situation of solving the problem, and it solves problem and is to provide the pattern formation method that correctly can form the organic electroluminescent device of the luminous pattern of the grade of the luminosity with expectation.
For solving the means of problem
In order to solve the above-mentioned problem that the present invention relates to, the reason etc. of the problems referred to above is studied, found that: when irradiating light, based on for penetrate because of illumination the organic function layer caused function change reciprocity failure characteristic, using the intensity of light and irradiation time at least any one controls as variable factor, form described luminous pattern, correctly can form the luminous pattern of the grade of the luminosity with expectation thus.
That is, the above-mentioned problem that the present invention relates to, solves by following scheme.
1. a pattern formation method for organic electroluminescent device, is characterized in that, it is for forming the pattern formation method of the organic electroluminescent device of luminous pattern to the organic electroluminescent device irradiation light possessing organic function layer between pair of electrodes,
When irradiating light, based on for penetrate because of illumination the above-mentioned organic function layer caused function change reciprocity failure characteristic, using the intensity of light and irradiation time at least any one carries out controlling as variable factor and forms above-mentioned luminous pattern.
2. the pattern formation method of the organic electroluminescent device according to the 1st, it is characterized in that, measure in advance based on the mutual relation for the above-mentioned variable quantity of function and the intensity of light and irradiation time of penetrating the above-mentioned organic function layer caused because of illumination and the above-mentioned reciprocity failure characteristic obtained, by the intensity of light and irradiation time at least any one carries out controlling and forms above-mentioned luminous pattern.
3. the pattern formation method of the organic electroluminescent device according to the 1st or the 2nd, is characterized in that, above-mentioned change of penetrating the function of the above-mentioned organic function layer caused because of illumination corresponds to the change of luminosity of above-mentioned organic electroluminescent device.
4. the pattern formation method of the organic electroluminescent device according to any one of the 1st ~ the 3rd, is characterized in that, the irradiation time of above-mentioned light be set to necessarily, makes the Strength Changes of this light and form above-mentioned luminous pattern.
5. the pattern formation method of the organic electroluminescent device according to any one of the 1st ~ the 3rd, is characterized in that, the intensity of above-mentioned light be set to necessarily, makes the irradiation time of this light change and form above-mentioned luminous pattern.
6. the pattern formation method of the organic electroluminescent device according to any one of the 1st ~ the 5th, is characterized in that, injects the description of row point and form above-mentioned luminous pattern by above-mentioned illumination.
7. the pattern formation method of the organic electroluminescent device according to any one of the 1st ~ the 5th, is characterized in that, by penetrating the intensity that adjusts above-mentioned light via the above-mentioned illumination of pattern formation mask and forming above-mentioned luminous pattern.
The effect of invention
According to the present invention, the pattern formation method that correctly can form the organic electroluminescent device of the luminous pattern of the grade of the luminosity with expectation can be provided.
For performance mechanism and even the mechanism of action of effect of the present invention, as following.
With regard to the pattern formation method of organic electroluminescent device that the present invention relates to, when irradiating light, based on for penetrate because of illumination the organic function layer caused function change reciprocity failure characteristic, using the intensity of light and irradiation time at least any one carries out controlling as variable factor and forms luminous pattern, therefore suitably can determine intensity and the irradiation time of the light corresponding to the luminosity expected, correctly can form the luminous pattern of the grade of the luminosity with expectation.
In addition, according to the present invention, suitably can determine the intensity of light and the irradiation time that correspond to the luminosity expected, the illumination therefore can carrying out organic electroluminescent device with the accumulated light of necessary irreducible minimum is penetrated, and the pattern that can carry out organic electroluminescent device is expeditiously formed.
Accompanying drawing explanation
Fig. 1 is the chart of the relation of the relative luminous brightness of accumulated light when having irradiated the light of wavelength 404nm with the intensity of different light to organic EL element and organic EL element.
Fig. 2 is the chart of the relation of the relative luminous brightness of accumulated light when having irradiated the light of wavelength 365nm with the intensity of different light to organic EL element and organic EL element.
Fig. 3 is the chart of the relation of the relative luminous brightness of accumulated light when having irradiated the light of wavelength 385nm with the intensity of different light to organic EL element and organic EL element.
Fig. 4 is for representing the chart of the intensity of light required for the pattern obtaining relative luminous brightness 0.1 and the relation of irradiation time.
The intensity of light of Fig. 5 required for the pattern in order to obtain each relative luminous brightness and the graph of a relation of irradiation time.
Fig. 6 represents relative to the intensity D of light of each relative luminous brightness and the figure of irradiation time t.
Fig. 7 is the schematic configuration diagram of luminous pattern forming apparatus.
Fig. 8 represents relative to the irradiation power P of the LD light source of each relative luminous brightness and the figure of LD electric current I
Fig. 9 represents the figure relative to the light transmittance T of each relative luminous brightness.
Embodiment
The feature of the manufacture method of organic electroluminescent device of the present invention is, when irradiating light, based on for penetrate because of illumination the above-mentioned organic function layer caused function change reciprocity failure characteristic, using the intensity of light and irradiation time at least any one carries out control as variable factor and forms above-mentioned luminous pattern.This is characterized as the common technical characteristic of the invention that relates to each side of the present invention the 1st aspect ~ the 7th aspect.
In addition, the present invention be preferably based on the mutual relation of the above-mentioned variable quantity of function and the intensity of light and irradiation time of penetrating the above-mentioned organic function layer caused because of illumination measured in advance and the above-mentioned reciprocity failure characteristic obtained, to the intensity of light and irradiation time at least any one controls and forms above-mentioned luminous pattern.Thus, suitably can determine intensity and the irradiation time of the light corresponding to the luminosity expected, correctly can form the luminous pattern of the grade of the luminosity with expectation.
In addition, the irradiation time of above-mentioned light is preferably set to necessarily, makes the Strength Changes of this light and form luminous pattern by the present invention.Thus, such as, irradiated the situation forming above-mentioned luminous pattern by laser inferior, can use existing irradiation position scanning technique, the pattern that easily can carry out organic EL element is formed, and can reduce the cost that pattern is formed simultaneously.
In addition, the intensity of above-mentioned light is preferably set to necessarily, makes the irradiation time of this light change and form above-mentioned luminous pattern by the present invention.Thus, owing to not needing the Strength Changes making light, therefore do not need photodetector, the amplifier in the supervision of luminous intensity with wide dynamic range, good S/N ratio.Therefore, the cost reduction that the pattern that easily can carry out organic EL element is formed, pattern can be made to be formed simultaneously.
In addition, the present invention forms above-mentioned luminous pattern preferably by above-mentioned illumination injects the description of row point.Thus, luminous pattern can be formed accurately to organic electroluminescent device.
In addition, the present invention penetrates preferably by the above-mentioned illumination via pattern formation mask the intensity that adjusts above-mentioned light and forms above-mentioned luminous pattern.Thus, easily luminous pattern can be formed to organic electroluminescent device.
Below, to the present invention and its inscape and be described in detail for implementing mode form of the present invention.Be explained, in this application, " ~ " is to use containing the implication of numerical value described before and after it as lower limit and higher limit.
" formation of organic electroluminescent device "
In the present invention, following for organic electroluminescent device (hereinafter also referred to as " organic EL element ".) formation be described.
With regard to organic EL element, substrate stacks gradually the 1st electrode, organic function layer and the 2nd electrode and forms.In addition, also can be formed as follows: arrange in the end of the 1st electrode and take out electrode and via this taking-up electrode, external power source (omitting diagram) be connected to the 1st electrode.The mode that organic EL element is taken out from substrate-side or its opposing face side with luminous light is formed.
The Rotating fields of organic EL element is not particularly limited, and can be known general Rotating fields.Such as, the 1st electrode plays function as positive pole (i.e. anode), the 2nd electrode plays function as negative pole (i.e. negative electrode).Now, such as, organic function layer can be formed and stack gradually the formation of hole injection layer/hole transmission layer/luminescent layer/electron transfer layer/electron injecting layer from the 1st electrode side as positive pole, but the luminescent layer needing at least there is use organic material and constitute.Hole injection layer and hole transmission layer can be arranged as hole transport implanted layer, and electron transfer layer and electron injecting layer can be arranged as electric transmission implanted layer.In addition, in these organic function layers, such as electron injecting layer is also made up of inorganic material sometimes.
In addition, organic function layer also can be the also stacked formation of hole blocking layer, electronic barrier layer etc. at necessity place as required except these layers.And then luminescent layer also can form the assorted luminescent layer with the luminous light producing each wavelength region may, the formation making these assorted luminescent layers stacked via the intermediate layer of non-luminescent.Intermediate layer also can play function as hole blocking layer, electronic barrier layer.
In addition, also can be stepped construction as required as the 2nd electrode of negative pole.In addition, for the purpose of the low resistance realizing the 1st electrode, also can connect with the 1st electrode and auxiliary electrode is set.
In such formation, only become the light-emitting zone of organic EL element by the part (from stacked direction, the region of the 1st electrode, organic function layer and the 2nd electrode overlap) that the 1st electrode and the 2nd electrode have clamped organic function layer.
With regard to organic EL element configured as described above, for the purpose of the deterioration of the organic function layer constituted to prevent from using organic material etc., substrate seals with encapsulant described later.But the terminal part of the 1st electrode, the 2nd electrode or taking-up electrode is exposed from encapsulant with the state maintaining mutually insulating properties on substrate.
For organic EL element configured as described above, by following pattern formation method, form the luminous pattern with the grade of the luminosity of expectation.
" pattern formation method of organic EL element "
(1) reciprocity failure characteristic
First, the discoveries such as the present inventor: when having carried out pattern formation when being penetrated by illumination organic EL element, as shown in fig. 1, for the function of organic function layer relative to the variable quantity of the accumulated light of the light irradiated in organic EL element, reciprocity failure is produced.Be explained, if the function of organic function layer changes because illumination is penetrated, then according to its variable quantity, the luminosity of organic EL element also changes.
At this, in the present invention so-called " reciprocity law ", if to refer to according to the accumulated light amassed as the intensity of the light irradiated and irradiation time necessarily, Bu Sen-Rothko rule that the variable quantity of organic function layer is also certain.In addition, in the present invention so-called " reciprocity failure ", if to refer to according to the accumulated light as the intensity of the light irradiated and the long-pending of irradiation time necessarily, the reciprocity law that the variable quantity of organic function layer is also certain is false.In addition, in the present invention so-called " reciprocity failure characteristic ", for the relation of the intensity of light and the variable quantity of irradiation time and organic function layer, refer to that the intensity of light and irradiation time produce reciprocity failure when getting any value, also can comprise the region that part reciprocity law is set up.
Fig. 1 be represent using the semiconductor laser of wavelength 404nm as the light of light source, each setting intensity, measure the chart of the result of the relative luminous brightness of the organic EL element relative to accumulated light.With regard to the relative luminous brightness of the organic EL element in the present invention, the state (being equivalent to white brightness) that organic function layer does not change completely by not irradiating light is completely set to 1, sets each relative luminous brightness.In addition, irradiate light and organic function layer changes, the reduction of luminosity reaches the limit state is equivalent to black brightness, be about 0.1 in this mensuration.In addition, with regard to the irradiation of light, the organic EL element self-induced transparency substrate-side after sealing is carried out.In addition, in FIG, for the intensity (W/cm of the light that will irradiate in organic EL element
2) be set to 7.6W/cm
2, 19.5W/cm
2, 40.4W/cm
2, 59.2W/cm
2, 470.0W/cm
2, 23083.0W/cm
2each situation of situation, the measurement result of the relative luminous brightness of the organic EL element relative to accumulated light is shown.
Clear and definite by Fig. 1, even if the accumulated light irradiated in the light of organic EL element is identical value, when the intensity of light is different, the relative luminous brightness of organic EL element is also different.Thus, illustrate: when utilizing light-struck pattern to be formed to organic EL element, even if accumulated light is certain, when the intensity of light is different with irradiation time, relative luminous brightness also difference, i.e. the generation reciprocity law timeliness of organic function layer.
In addition, illustrated by the measurement result shown in Fig. 1: the intensity of light is larger, more can obtain the pattern of the relative luminous brightness expected with little accumulated light.
In addition, as shown in Fig. 2 and Fig. 3, confirm: even if when light source is set to wavelength 365nm, wavelength 385nm LED (LightEmittingDiode), also find identical characteristic.The relative luminous brightness of the organic EL element of the accumulated light of the intensity relative to each light when Fig. 2 illustrates the LED employing wavelength 365nm, the relative luminous brightness of the organic EL element of the accumulated light of the intensity relative to each light when Fig. 3 illustrates the LED employing wavelength 385nm.
(2) based on the pattern formation method of reciprocity failure characteristic
Based on knowledge opinion as above, in the pattern formation method of organic electroluminescent device of the present invention, be characterised in that, when irradiating light, based on to penetrate because of illumination the organic function layer caused function change reciprocity failure characteristic, using the intensity of light and irradiation time at least any one carries out control as variable factor and forms luminous pattern.Below an example of its concrete method is described.
First, for each relative luminous brightness of the organic EL element changed because illumination is penetrated, exported as the pattern obtaining this relative luminous brightness respectively and the intensity of light needed and the relation of irradiation time.Such as, in Fig. 4, be depicted as the pattern obtaining relative luminous brightness 0.1 and the intensity of light needed and the relation of irradiation time with log-log graph.Be explained, Fig. 4 illustrates each situation for the light source employing wavelength 365nm, 404nm, has carried out illumination penetrate from transparent substrate side to the organic EL element after sealing.
In example in the diagram, being set to Y in the irradiation time of the light needed by the pattern in order to obtain relative luminous brightness 0.1, the intensity of light is when being set to X, when employing the light source of wavelength 404nm, becoming Y=2.47 × 10
4x
-1.67.In addition, when employing the light source of wavelength 365nm, Y=9.15 × 10 are become
2x
-1.61.Illustrate like this: the situation employing the light source of wavelength 365nm, can with the intensity of less light and shorter irradiation time obtains the pattern of relative luminous brightness 0.1 compared with the situation of the light source employing wavelength 404nm.
When the luminous pattern formed being penetrated by illumination is represented with 256 grades of 8bit, as shown in Figure 5, relative luminous brightness 1 ~ 0.1 carried out 256 deciles, measured halved in order to the intensity of the pattern and the light needed that obtain each relative luminous brightness and irradiation time, derive the intensity of light and the relation of irradiation time respectively.The intensity of light that Fig. 5 needs in order to the pattern obtaining each relative luminous brightness and the graph of a relation of irradiation time.
Then, as shown in Figure 6 each relative luminous brightness is arranged to intensity and the irradiation time of light.Fig. 6 represents relative to the intensity D of light of each relative luminous brightness and the figure of irradiation time t.
Such as, when wanting the pattern obtaining relative luminous brightness 0.1, can with the intensity D of light
000and irradiation time t
000carry out the irradiation of light, its intensity D
000and irradiation time t
000the arbitrary value on the curve (on log-log graph roughly straight line) of the relative luminous brightness 0.1 shown in Fig. 5 can be got.Equally, even if when wanting the pattern of each relative luminous brightness obtaining other, can carry out the irradiation of light with the intensity D of the light shown in Fig. 6 and irradiation time t, its intensity D and irradiation time t can get the arbitrary value on the curve of each relative luminous brightness shown in Fig. 5.
When wanting the pattern obtaining each relative luminous brightness, the intensity D of light and irradiation time t is set as arbitrary value, or can according to the formation of light irradiation device, the suitable setting of light illuminating method.Such as, as described later, the light-emitting area of organic EL element is carried out scanning with certain speed in light irradiation position and under carrying out light-struck situation with a description thus, the irradiation time of the light relative to each relative luminous brightness is all set as identical value, determined to correspond to the intensity of the light of each relative luminous brightness by the chart shown in Fig. 5.
Be explained, in order to ensure the contrast of the pattern of relative luminous brightness 1 and the pattern of relative luminous brightness 0.1, the intensity D of light
255with irradiation time t
255preferably be set to 0 respectively.
With the intensity of the light relative to each relative luminous brightness that have thus determined and irradiation time, the irradiation light-emitting area of organic EL element, each region being carried out to light, the light-emitting area of organic EL element forms the luminous pattern of expectation.
Be explained, carry out light-struck opportunity for organic EL element, can after with encapsulant sealing organic el element, also can the arbitrary layer formed in each layer of organic function layer has just been carried out stacked after.
In addition, just organic EL element is carried out with regard to light-struck direction, if light can be made to arrive organic function layer and change the function of this organic function layer, then can irradiate from substrate-side, also can irradiate from its opposing face side.But, in organic EL element, be located at the substrate of light incident side, electrode etc. be preferably made up of translucent material.
(3) pattern formation method utilizing point to describe and patterning device
At this, referring to Fig. 7 to carry out organic EL element of the present invention pattern formation method in the patterning device 1 that preferably uses be described.
Fig. 7 is the schematic configuration diagram of the patterning device 1 can implementing pattern formation method of the present invention.Patterning device 1 forms the some drawing apparatus of luminous pattern for forming small some mark (De ッ ト マ ー Network) in organic EL element 2.
Patterning device 1 possesses: the semiconductor laser (LD of the laser of injection specific wavelength, LaserDiode) light source 11, the light penetrated from this LD light source 11 is made to be the collimating lens 12 of directional light, the light being formed as directional light by collimating lens 12 is focused to the collector lens 13 of the spot diameter of regulation, reflect the beam splitter 14 of a part for the light penetrated from collimating lens 12, the photodetector 15 of the intensity of the light that detection is reflected by beam splitter 14, by the speculum 16 that the light penetrated from collector lens 13 reflects to organic EL element 2, the adjustment part 17 of the gradient of adjustment speculum 16, and control the control part 18 etc. of each parts.
By such patterning device 1, first, with regard to control part 18, the view data inputted by never illustrated external equipment (such as PC, various server or printer etc.) generates the luminosity data of the luminosity of each coordinate representing this image.
Then, with regard to control part 18, intensity and/or the irradiation time of the light required in the some mark forming the relative luminous brightness expected is calculated.
At this, with regard to patterning device 1, form as follows: for each point mark, be set to the irradiation time of light necessarily, make the Strength Changes of light, form the some mark of the luminosity of expectation thus.By forming in this wise, known scanning technique can be used.Therefore, the luminous pattern that easily can carry out employing patterning device 1 is formed, and can reduce the manufacturing cost of patterning device 1 simultaneously.
Therefore, the irradiation time of the light relative to each relative luminous brightness is all set as such as 1ms, selects the intensity of the light required in the some mark forming each relative luminous brightness by control part 18.The irradiation power P [mW] that control part 18 calculates the light in order to penetrate from LD light source 11 by the intensity of the light corresponding to each relative luminous brightness and electric current (LD electric current) I [mA] (with reference to Fig. 8) that should apply in order to the light penetrating this irradiation power P.Be explained, in the example in fig. 8, in order to form relative luminous brightness 1 some mark required for LD electric current I be 0, if but lower than the threshold value of LD light source 11, then also can not be 0.
Then, control part 18 adjusts the gradient of speculum 16 around the every 1ms of 2 axle by adjustment part 17, light irradiation position in organic EL element in X direction and Y-direction scanning while based on the above-mentioned luminosity data generated will the output of pulse signal of value of LD electric current of each coordinate of expression to LD light source 11.LD light source 11, based on have input pulse signal, injection laser, can form multiple mark thus and form the luminous pattern expected in organic EL element.Be explained, with regard to control part 18, when carrying out illumination and penetrating, detected the intensity of the reverberation utilizing beam splitter 14 to obtain by photodetector 15, monitor the data that have detected.Thus, control part 18 when the intensity of the light penetrated from LD light source 11 produces error in the change because of temperature humidity environment etc., can be revised the LD electric current I that applies LD light source 11 and correctly penetrate the intensity of the light of expectation.
Be explained, in above-mentioned patterning device 1, the irradiation time of light be set to 1ms, but be not limited to this value.
In addition, in above-mentioned patterning device 1, the irradiation time of light is set to necessarily, makes the Strength Changes of light and form the some mark of the relative luminous brightness of expectation, but also the intensity of light can be set to certain and irradiation time is changed.Now, do not need with the intensity of wide range detection light, photodetector 15, exported carry out IV conversion, the not shown amplifier that carries out amplifying do not need to use the part with wide dynamic range and good S/N ratio, therefore can reduce the cost of patterning device 1.
And then, in above-mentioned patterning device 1, the irradiation time of light is set to necessarily, makes the Strength Changes of light and form the some mark of the relative luminous brightness of expectation, but also can make the intensity of light and irradiation time change simultaneously.
(4) pattern formation method of mask is employed
In addition, as the pattern formation method of organic EL element of the present invention, the pattern being not limited to utilize above-mentioned point to describe is formed, and also can be formed for the pattern employing pattern formation mask.
In the pattern formation method using mask, the luminous pattern of the expectation intensity of the light penetrated from light source and irradiation time are set to necessarily, formed corresponding to organic EL element, via set each region light transmittance mask and carry out illumination and penetrate.That is, the mask by using light transmittance different in each region, at the intensity of each Region control to the light that organic EL element is irradiated, the luminous pattern of formation expectation.
The light transmittance in each region of mask sets as shown in Figure 9.The light transmittance of the mask shown in Fig. 9 is derived by the intensity of light in each relative luminous brightness shown in Fig. 5 and the graph of a relation of irradiation time.
That is, in the method for such as above-mentioned use mask, because the irradiation time of light is set as setting, therefore in order to obtain each relative luminous brightness pattern required for the intensity of light determined by the chart shown in Fig. 5.With regard to the light transmittance T of the mask required for the pattern in order to obtain each relative luminous brightness, if the intensity of the light to organic EL element irradiation required for the pattern in order to obtain this relative luminous brightness is set to D, the intensity of the light irradiated mask is set to Dmsk, then represented by T=D/Dmsk.Therefore, need to be at least than the intensity D in order to obtain the light required for each relative luminous brightness to the intensity Dmsk of the light that mask irradiates
000~ D
255any one large value or with each relative luminous brightness D
000~ D
255in the identical value of maximum value.
Be explained, be easy to viewpoint from making the making of mask and consider, the light transmittance preferably in the mask needed for the pattern obtaining relative luminous brightness 1 is 0%.
By the mask configuration that will constitute as mentioned above in organic EL element light-emitting area, with the intensity of regulation and irradiation time, the irradiation of light is carried out to organic EL element via this mask, the luminous pattern of expectation can be formed in organic EL element.
(5) intensity of light and irradiation time
Then, illustrate and the light-struck intensity in above-mentioned pattern formation method and irradiation time is described.
As shown in fig. 1, the intensity of carrying out the light irradiated is larger, and more can form the pattern of the relative luminous brightness expected with little accumulated light, the intensity therefore more increasing light more can shorten irradiation time tremendously.
Such as, carrying out in the light-struck situation utilizing point to describe, when the emission wavelength of light source is set to 404nm, then by Fig. 4, if the intensity of light is set to 26kW/cm
2above, then 1 of relative luminous brightness 0.1 irradiation time marked can be made to be below 1ms, luminous pattern can be formed with very high speed.When being set to resolution 200dpi, then 1 mark is of a size of 25.4mm/200=0.127mm, therefore when the demifacet of the organic EL element by effective light-emitting zone 100mm × 100mm is set to non-luminescent (relative luminous brightness 0.1), description is counted as (description region 100mm × 100mm × 0.5)/(some label size 0.127mm × 0.127mm)=310000 points, the description time is 310000 × 1ms=310s=5.2min, becomes about 5 minutes such very short time.
In addition, if shorten the wavelength carrying out the light irradiated, then the pattern that can carry out further is at short notice formed.
Such as, when using the light source of wavelength 365nm, by Fig. 4,1 mark irradiation time of relative luminous brightness 0.1 is the intensity of the light of 1ms is 4.8kW/cm
2.
Therefore, relative to wavelength X, irradiation time is the pass of the intensity D of the light of 1ms is D [W/cm
2]=550 λ [nm]-1.96 × 10
5.Therefore, when the pattern utilizing point to describe is formed, if be 550 λ [nm]-1.96 × 10 by the intensity settings of light
5above, then pattern can be formed with very high speed.Be explained, Fig. 4 illustrate the transmitance for the light of the duplexer by substrate and the 1st electrode be 70% organic EL element carried out the result of light-struck situation, the intensity therefore as the light irradiated luminescent layer can be set as 385 λ [nm]-1.37 × 10
5above.
On the other hand, in using the pattern of mask to be formed, if use commercially available general UV exposure device to carry out pattern formation, then the intensity of the light of this device is tens of ~ hundred mW/cm
2left and right, therefore, need the irradiation time of more than 10h, production efficiency is poor.At this, as mentioned above, in the pattern of organic EL element is formed, more increase the intensity of carrying out the light irradiated and more can improve irradiation time, if therefore carry the illuminator of multiple wavelength 365nm and the intensity of light is set to 0.43W/cm tremendously
2above, then irradiation time can be made to be below 1h, significantly can to improve treating capacity.
When to calculate for wavelength X irradiation time in the same manner as with the pattern that above-mentioned point is described is formed be the relation of the intensity D of the light of 1h, be then D [W/cm
2]=0.070 λ [nm]-25.Therefore, when using the pattern of mask to be formed, if by the intensity settings of light be 0.070 λ [nm] more than-25, even if then utilizing the pattern of the wavelength beyond ultraviolet range to be formed, also can productivity ratio be guaranteed.Be explained, as the intensity of the light irradiated luminescent layer, can be set as that 0.049 λ [nm] is more than-17.5.
Below, the details of main each layer of the organic EL element of above-mentioned pattern formation method of the present invention can be carried out and its manufacture method is described to forming.
" substrate "
As the substrate that can use in organic EL element of the present invention, can glass, plastics etc. be enumerated, be not particularly limited, in addition, can be transparent also can for opaque.As the transparent substrate that can preferably use, can enumerate: glass, quartz, transparent resin film.Be particularly preferably and can give flexible resin molding to organic EL element.
As the thickness of substrate, being not particularly limited, can be arbitrary thickness.
As resin molding, such as can enumerate: PETG (PET), the polyester of PEN (PEN) etc., polyethylene, polypropylene, cellophane, cellulose diacetate, cellulosic triacetate (TAC), cellulose acetate butyrate, cellulose acetate propionate (CAP), CAP, the cellulose esters of cellulose nitrate etc. or their derivative, Vingon, polyvinyl alcohol, poly ethylene vinyl alcohol, syndiotactic polystyrene, Merlon, norbornene resin, polymethylpentene, polyether-ketone, polyimides, polyether sulfone (PES), polyphenylene sulfide, polysulfones, Polyetherimide, polyether-ketone acid imide, polyamide, fluororesin, nylon, polymethyl methacrylate, acrylic compounds or polyarylate class, ア ー ト Application (trade name JSR Inc.) or the such cyclic olefine resin etc. of ア ペ Le (trade name Mitsui Chemicals, Inc. system).
On the surface of resin molding, also can be formed by inorganic matter or organic substance or the gas barrier film that forms both it.As such gas barrier film, the such as steam permeability (25 ± 0.5 DEG C, relative humidity (90 ± 2) %RH) be preferably with the method according to JISK7129-1992 determines is 0.01g/ (m
224h) following gas barrier film is more preferably 10 with the oxygen permeability that the method according to JISK7126-1987 determines
-3ml/ (m
224hatm) below, steam permeability is 10
-5g/ (m
224h) following high gas-obstructing character film.
As the material forming gas barrier film, such as, as long as having the material suppressing moisture, oxygen etc. to bring the function of the immersion of the material of the deterioration of element, silica, silicon dioxide, silicon nitride etc. can be used.And then, in order to improve the fragility of this film, the stepped construction of layer that more preferably there are these inorganic layers and be made up of organic material.The lamination order of inorganic layer and organic layer is not particularly limited, but preferably that both are repeatedly alternately laminated.
Formation method for gas barrier film is not particularly limited, such as can use vacuum vapour deposition, sputtering method, reactive sputtering method, molecular beam epitaxy, cluster ions bundle method, ion plating method, Plasma Polymerization, atmospheric pressure plasma polymerization, plasma CVD method, laser CVD method, thermal cvd, cladding process etc., but particularly preferably utilize such atmospheric pressure plasma polymerization described in Japanese Unexamined Patent Publication 2004-68143 publication.
As opaque supporting substrates, such as, can enumerate: the metallic plate, opaque resin substrate, ceramic substrate etc. of aluminium, stainless steel etc.
" the 1st electrode "
With regard to the 1st electrode, spendable all electrodes in organic EL element usually can be used.Specifically, can enumerate: aluminium, silver, magnesium, lithium, magnesium/copper mixture, magnesium/silver-colored mixture, magnesium/aluminium mixture, magnesium/indium mixture, indium, lithium/aluminium mixture, rare earth metal, ITO, ZnO, TiO
2, SnO
2deng oxide semiconductor etc.
In the present invention, the 1st electrode is preferably transparency electrode, more preferably transparent metal electrode.Be explained, so-called the transparent of 1st electrode refers to that the light transmittance under wavelength 550nm is more than 50%.
As the formation method of the 1st electrode, such as, can be suitable for using known spin coating, vapour deposition method, sputtering method etc., as its patterning process, such as, according to circumstances can use and knownly utilize the composition of photoetching, utilize the composition etc. of pattern mask.When taking out luminous light from the 1st electrode, preferably make transmitance be greater than 10%, in addition, the sheet resistance as the 1st electrode is preferably hundreds of Ω/below.
And then, although the thickness of the 1st electrode also depends on material, usually at 10 ~ l000nm, preferably select in the scope of 10 ~ 200nm.
1st electrode also can be formed as the electrode of 2 Rotating fields be made up of the basalis defined on substrate and the electrode layer that defines thereon.Wherein, electrode layer such as can use and utilize silver or the layer that constitutes as the alloy of main component using silver, and basalis such as can use and utilize the compound containing nitrogen-atoms and the layer that constitutes.Be explained, in electrode layer, so-called main component refers to that the content in electrode layer is more than 98 quality %.
" organic function layer (light emitting functional layer) "
(1) luminescent layer
At least containing luminescent layer in organic function layer.
Phosphorescence luminance compound is contained as luminescent material in the luminescent layer used in the present invention.Be explained, in luminescent layer, also can contain multiple phosphorescence luminance compound.In addition, as luminescent material, can fluorescent material be used, also can be used together phosphorescence luminance compound and fluorescent material.
This luminescent layer is the electronics that is filled with from the 2nd electrode or electron transfer layer and carries out luminous layer from the hole-recombination that the 1st electrode or hole transmission layer are filled with, carrying out luminous part can, in the layer of luminescent layer, also can be the interface of the layer adjoined with luminescent layer.
As such luminescent layer, as long as contained luminescent material meets luminous important document, its formation is not particularly limited.In addition, there is identical luminescent spectrum, the layer of luminous greatly wavelength also can be multilayer.Now, preferably there is between each luminescent layer the intermediate layer (omitting diagram) of non-luminescent.
The summation of the thickness of luminescent layer preferably in the scope of 1 ~ 100nm, from the viewpoint of more low driving voltage can be obtained, more preferably in the scope of 1 ~ 30nm.
Be explained, the summation of the thickness of so-called luminescent layer, when there is the intermediate layer of non-luminescent when between luminescent layer, for also comprising the thickness in this intermediate layer.
When by the luminescent layer that multilayer is formed, as the thickness of each luminescent layer, be preferably adjusted in the scope of 1 ~ 50nm, be more preferably adjusted in the scope of 1 ~ 20nm further.When stacked multiple luminescent layers carry out luminescence with each blue, green, red illuminant colour, the relation for the thickness of each luminescent layer is not particularly limited.
As above luminescent layer, known luminescent material, host compound such as can be carried out film forming by the known film forming method of vacuum vapour deposition, spin-coating method, the tape casting, LB method, ink-jet method etc. and formed.
At this, in the present invention, as the concrete example of the phosphorescence luminance compound preferably used in the luminescent layer of organic EL element, compound etc. described in the following literature can be enumerated.
Can enumerate: Nature395, 151 (1998), Appl.Phys.Lett.78, 1622 (2001), Adv.Mater.19, 739 (2007), Chem.Mater.17, 3532 (2005), Adv.Mater.17, 1059 (2005), No. 2009/100991st, International Publication, No. 2008/101842nd, International Publication, No. 2003/040257th, International Publication, U.S. Patent Publication No. 2006/835469 specification, U.S. Patent Publication No. 2006/0202194 specification, U.S. Patent Publication No. 2007/0087321 specification, the compound recorded in U.S. Patent Publication No. 2005/0244673 specification etc.
In addition, can enumerate: Inorg.Chem.40, 1704 (2001), Chem.Mater.16, 2480 (2004), Adv.Mater.16, 2003 (2004), Angew.Chem.lnt.Ed.2006, 45, 7800, Appl.Phys.Lett.86, 153505 (2005), Chem.Lett.34, 592 (2005), Chem.Commun.2906 (2005), Inorg.Chem.42, 1248 (2003), No. 2009/050290th, International Publication, No. 2009/000673rd, International Publication, United States Patent (USP) No. 7332232 specification, No. 2009/0039776th, U.S. Patent Publication, United States Patent (USP) No. 6687266 specification, U.S. Patent Publication No. 2006/0008670 specification, U.S. Patent Publication No. 2008/0015355 specification, United States Patent (USP) No. 7396598 specification, U.S. Patent Publication No. 2003/0138657 specification, the compound recorded in United States Patent (USP) No. 7090928 specification etc.
In addition, also can enumerate: Angew.Chem.lnt.Ed.47, 1 (2008), Chem.Mater.18, 5119 (2006), Inorg.Chem.46, 4308 (2007), Organometallics23, 3745 (2004), Appl.Phys.Lett.74, 1361 (1999), No. 2006/056418th, International Publication, No. 2005/123873rd, International Publication, No. 2005/123873rd, International Publication, No. 2006/082742nd, International Publication, U.S. Patent Publication No. 2005/0260441 specification, United States Patent (USP) No. 7534505 specification, U.S. Patent Publication No. 2007/0190359 specification, United States Patent (USP) No. 7338722 specification, United States Patent (USP) No. 7279704 specification, the compound recorded in U.S. Patent Publication No. 2006/103874 specification etc.
And then, can also enumerate: the compound recorded in No. 2005/076380th, International Publication, No. 2008/140115th, International Publication, No. 2011/134013rd, International Publication, No. 2010/086089th, International Publication, No. 2012/020327th, International Publication, No. 2011/051404th, International Publication, No. 2011/073149th, International Publication, JP 2009-114086 publication, JP 2003-81988 publication, JP 2002-363552 publication etc.
In the present invention, as preferred phosphorescence luminance compound, can enumerate: the metal-organic complex at central metal with Ir.Further preferably, the complex compound preferably containing the coordination pattern of at least a kind in metal-carbon key, metal-nitrogen key, metal-oxygen key, metal-sulfur key.
As phosphorescence luminance compound (also referred to as phosphorescence photism metal complex), such as can by application OrganicLetter magazine, vol.3, No.16,2579 ~ 2581 pages (2001); Inorg.Chem. the 30th volume, No. 8,1685 ~ 1687 pages (1991 years); J.Am.Chem.Soc., 123 volumes, 4304 pages (calendar year 2001); InorganicChemistry, the 40th volume, No. 7,1704 ~ 1711 pages (calendar year 2001); InorganicChemistry, the 41st volume, No. 12,3055 ~ 3066 pages (2002 years); NewJournalofChemistry, the 26th volume, 1171 pages (2002); EuropeanJournalofOrganicChemistry, the 4th volume, 695 ~ 709 pages (2004); And in these documents in described list of references etc. disclosed method synthesize.
In addition, in the present invention, as the concrete example of the host compound preferably used in the luminescent layer of organic EL element, such as, can enumerate: Japanese Unexamined Patent Publication 2001-257076 publication, Japanese Unexamined Patent Publication 2001-357977 publication, Japanese Unexamined Patent Publication 2002-8860 publication, Japanese Unexamined Patent Publication 2002-43056 publication, Japanese Unexamined Patent Publication 2002-105445 publication, Japanese Unexamined Patent Publication 2002-352957 publication, Japanese Unexamined Patent Publication 2002-231453 publication, Japanese Unexamined Patent Publication 2002-234888 publication, Japanese Unexamined Patent Publication 2002-260861 publication, Japanese Unexamined Patent Publication 2002-305083 publication, U.S. Patent Publication No. 2005/0112407 specification, U.S. Patent Publication No. 2009/0030202 specification, No. 2001/039234th, International Publication, No. 2008/056746th, International Publication, No. 2005/089025th, International Publication, No. 2007/063754th, International Publication, No. 2005/030900th, International Publication, No. 2009/086028th, International Publication, No. 2012/023947th, International Publication, JP 2007-254297 publication, compound described in European Patent No. 2034538 specification etc., but the present invention is not limited to these.
(2) implanted layer (hole injection layer, electron injecting layer)
So-called implanted layer, it is the layer in order to driving voltage reduces, luminosity improves and is arranged between electrode and luminescent layer, recorded in detail in the 2nd volume the 2nd chapter " electrode material " (123 ~ 166 pages) of " organic EL element and its industrialization forefront (NTS corporation issues on November 30th, 1998) ", had hole injection layer and electron injecting layer.
Implanted layer can be arranged as required.If be hole injection layer, then may reside between anode and luminescent layer or hole transmission layer, if be electron injecting layer, then may reside between negative electrode and luminescent layer or electron transfer layer.
With regard to hole injection layer, in Japanese Unexamined Patent Publication 9-45479 publication, Japanese Unexamined Patent Publication 9-260062 publication, Japanese Unexamined Patent Publication 8-288069 publication etc., also there is it to record in detail, as concrete example, can enumerate: the phthalocyanine layer representated by copper phthalocyanine, the oxide skin(coating) representated by vanadium oxide, amorphous carbon layer, employ the macromolecule layer etc. of the electroconductive polymer of polyaniline (emeraldine), polythiophene etc.
With regard to electron injecting layer, in Japanese Unexamined Patent Publication 6-325871 publication, Japanese Unexamined Patent Publication 9-17574 publication, Japanese Unexamined Patent Publication 10-74586 publication etc., also there is it to record in detail, specifically, can enumerate: the representative metal level such as strontium, aluminium, the alkali halide layer representated by potassium fluoride, the alkali earth metallic compound layer representated by magnesium fluoride, oxide skin(coating) etc. representated by molybdenum oxide.Electron injecting layer of the present invention is preferably very thin film, although also depend on raw material, and the scope of preferred 1nm ~ 10 of its thickness μm.
(3) hole transmission layer
Hole transmission layer is made up of the hole mobile material of the function with transporting holes, and broadly hole injection layer, electronic barrier layer are also included in hole transmission layer.Hole transmission layer can arrange single or multiple lift.
As hole mobile material, arbitrary performance of the block of the cuniculate injection of tool or transmission, electronics, organic substance, inorganic matter.Such as can enumerate: triazole derivative, oxadiazole derivative, imdazole derivatives, polyaryl alkane derivatives, pyrazoline derivative and pyrazolone derivative, phenylenediamine derivative, arylamine derivatives, amino replacement chalcone derivative, oxazole derivative, styrylanthracene derivatives, fluorenone derivatives, hydazone derivative, stilbene derivative, silazane derivatives, aniline based copolymer, in addition electroconductive polymer oligomer, particularly thiophene oligomers etc.
As hole mobile material, above-mentioned material can be used, preferably use porphyrin compound, aromatic uncle amine compound and styrylamine compounds, particularly preferably use aromatic uncle amine compound.
As the typical example of aromatic uncle amine compound and styrylamine compounds, can enumerate: N, N, N ', N '-tetraphenyl-4,4 '-diamino-phenyl; N, N '-diphenyl-N, N '-bis-(3-aminomethyl phenyl)-[1,1 '-biphenyl]-4,4 '-diamines (TPD); Two (4-bis--p-methylphenyl aminophenyl) propane of 2,2-; Two (4-bis--p-methylphenyl aminophenyl) cyclohexane of 1,1-; N, N, N ', N '-four-p-methylphenyl-4,4 '-benzidine; Two (4-bis--p-methylphenyl aminophenyl)-4-cyclohexylbenzene of 1,1-; Two (4-dimethylamino-2-aminomethyl phenyl) phenylmethane; Two (4-bis--p-methylphenyl aminophenyl) phenylmethane; N, N '-diphenyl-N, N '-two (4-methoxyphenyl)-4,4 '-benzidine; N, N, N ', N '-tetraphenyl-4,4 '-diaminodiphenyl ether; 4,4 '-bis-(diphenyl amino) quaterphenyl; N, N, N-tri-(p-methylphenyl) amine; 4-(two-p-methylphenyl is amino)-4 '-[4-(two-p-methylphenyl is amino) styryl] Stilbene; 4-N, N-diphenyl amino-(2-diphenylacetylene) benzene; 3-methoxyl group-4 '-N, N-diphenyl amino stibene (stilbenzene); The material in molecule with 2 fused aromatic rings, such as 4 recorded in N-phenyl carbazole and United States Patent (USP) No. 5061569 specification, three triphenylamine units recorded in 4 '-bis-[N-(1-naphthyl)-N-phenyl amino] biphenyl (NPD), Japanese Unexamined Patent Publication 4-308688 publication connect for star burst type 4,4 ', 4 "-three [N-(3-aminomethyl phenyl)-N-phenyl amino] triphenylamine (MTDATA) etc.
And then can use and these materials have been imported macromolecular chain or using the macromolecular material of these materials as high molecular main chain.In addition, the inorganic compound of p-type-Si, p-type-SiC etc. also can use as hole-injecting material, hole mobile material.
In addition, also can use as Japanese Unexamined Patent Publication 11-251067 publication, J.Huang etc., AppliedPhysicsLetters, 80 (2002), the p.139 middle so-called p-type hole mobile material recorded.In the present invention, from the viewpoint of more high efficiency light-emitting component can be obtained, preferably use these materials.
With regard to hole transmission layer, can by above-mentioned hole mobile material such as being carried out filming by the known method of vacuum vapour deposition, spin-coating method, the tape casting, the print process comprising ink-jet method, LB method etc. and being formed thus.Thickness for hole transmission layer is not particularly limited, and about being generally 5nm ~ 5 μm, is preferably 5 ~ 200nm.This hole transmission layer can be by one kind or two or more 1 Rotating fields formed in above-mentioned material.
In addition, also in the material of hole transmission layer, p can be improved by impurity.As its example, can enumerate: Japanese Unexamined Patent Publication 4-297076 publication, Japanese Unexamined Patent Publication 2000-196140 publication, Japanese Unexamined Patent Publication 2001-102175 publication, J.Appl.Phys., material described in 95,5773 (2004) etc.
Like this, if improve the p of hole transmission layer, then the element of more low power consumption can be made, therefore preferably.
(4) electron transfer layer
Electron transfer layer is made up of the material of the function with transmission electronic, and broadly electron injecting layer, hole blocking layer (omitting diagram) are also contained in electron transfer layer.Electron transfer layer can be arranged with the form of the stepped construction of single layer structure or multilayer.
In the electron transfer layer of single layer structure and the electron transfer layer of stepped construction, as the electron transport material (doubling as hole barrier materials) forming the layer segment adjoined with luminescent layer, as long as have the electron transmission that is filled with from negative electrode to the function of luminescent layer.As such material, arbitrary compound can be selected use from known compound.Such as can enumerate nitro-substituted fluorene derivative, diphenylquinone derivatives, thio-pyrylium dioxide derivative, carbodiimides, fluorenylidenemethane derivatives, anthraquinone bismethane, anthracyclinone derivatives Ji oxadiazole derivative etc.And then state in oxadiazole derivative upper, the thiadiazoles derivative oxygen atom of oxadiazole rings being substituted by sulphur atom, the quinoxaline derivant with the quinoxaline ring known as electron withdraw group also can use as the material of electron transfer layer.And then also can use these materials have been imported macromolecular chain or using the macromolecular material of these materials as high molecular main chain.
In addition, metal complex, such as three (oxine) aluminium (Alq of oxine derivative
3), three (5,7-dichloro-8-hydroxyquinoline) central metal of aluminium, three (5,7-D-Br-8-HQ) aluminium, three (2-methyl-oxine) aluminium, three (5-methyl-oxine) aluminium, two (oxine) zinc (Znq) etc. and these metal complexs metal complex that is replaced with In, Mg, Cu, Ca, Sn, Ga or Pb also can use as the material of electron transfer layer.
In addition, also can preferably be used as the material of electron transfer layer by the compound that alkyl, sulfonic group etc. instead of without metal or metal phthalocyanine or their end.In addition, as luminescent layer material and illustrative distyrylpyrazine derivatives also can use as the material of electron transfer layer, same with hole injection layer, hole transmission layer, the inorganic semiconductor of N-shaped-Si, N-shaped-SiC etc. also can use as the material of electron transfer layer.
Electron transfer layer can by such as carrying out filming to be formed by the known method of vacuum vapour deposition, spin-coating method, the tape casting, the print process comprising ink-jet method, LB method etc. by above-mentioned material.Thickness for electron transfer layer is not particularly limited, and about being generally 5nm ~ 5 μm, is preferably 5 ~ 200nm.Electron transfer layer can be by one kind or two or more 1 Rotating fields formed in above-mentioned material.
In addition, also can in electron transfer layer impurity, improve n.As its example, can enumerate: Japanese Unexamined Patent Publication 4-297076 publication, Japanese Unexamined Patent Publication 10-270172 publication, Japanese Unexamined Patent Publication 2000-196140 publication, Japanese Unexamined Patent Publication 2001-102175 publication, J.Appl.Phys., material described in 95,5773 (2004) etc.And then preferably in electron transfer layer, contain potassium, potassium compound etc.As potassium compound, such as, potassium fluoride etc. can be used.If improve the n of electron transfer layer like this, then can make the element of more low power consumption.
In addition, as the material (electron-transporting compound) of electron transfer layer, also the material same with the material forming above-mentioned basalis can be used.Even if its for the electron transfer layer doubling as electron injecting layer also identical, the material same with the material forming above-mentioned basalis can be used.
(5) barrier layer (hole blocking layer, electronic barrier layer)
With regard to barrier layer, can arrange further except above-mentioned each functional layer as organic function layer.Such as have Japanese Unexamined Patent Publication 11-204258 publication, hole barrier (holeblock) layer described in Japanese Unexamined Patent Publication 11-204359 publication and " organic EL element and its industrialization forefront (NTS corporation issues on November 30th, 1998) " 237 pages etc.
So-called hole blocking layer, broadly has the function of electron transfer layer.Hole blocking layer is made up of the hole barrier materials that the ability of function, the simultaneously transporting holes with transmission electronic is significantly little, by transmission electronic, simultaneously blocking hole, the probability of recombination in electronics and hole can be made to improve.In addition, the formation of electron transfer layer described later can be used as the hole blocking layer that the present invention relates to as required.Hole blocking layer is preferably adjacent with luminescent layer and arrange.
On the other hand, so-called electronic barrier layer, broadly has the function of hole transporting layer.Electronic barrier layer is made up of the material that the ability of function, the simultaneously transmission electronic with transporting holes is significantly little, by transporting holes, simultaneously block electrons, the probability of recombination in electronics and hole can be made to improve.In addition, also the formation of hole transmission layer described later can be used as electronic barrier layer as required.As the thickness of the hole blocking layer that the present invention relates to, be preferably 3 ~ 100nm, more preferably 5 ~ 30nm.
" the 2nd electrode "
2nd electrode is the electrode film playing function as the negative pole to organic function layer supply electronics, can use conductive compound and their mixture of metal, alloy, organic or inorganic.Specifically, can enumerate: aluminium, silver, magnesium, lithium, magnesium/copper mixture, magnesium/silver-colored mixture, magnesium/aluminium mixture, magnesium/indium mixture, indium, lithium/aluminium mixture, rare earth metal, ITO, ZnO, TiO
2, SnO
2deng oxide semiconductor etc.
2nd electrode makes by these conductive materials are formed film by the method for evaporation, sputtering etc.In addition, the sheet resistance as the 2nd electrode is preferably hundreds of Ω/below, and thickness is selected usually in the scope of 5 ~ 5000nm, preferably in the scope of 5 ~ 200nm.
Be explained, if if this organic EL element is the situation of taking out luminous light from the 2nd electrode side, as long as the conductive material then selecting light transmission good from above-mentioned conductive material forms the 2nd electrode.Now, above-mentioned pattern formation method is carried out by irradiating light from the 2nd electrode side.
" taking-up electrode "
Take out electrode the 1st electrode and external power source are electrically connected, as its material, be not particularly limited, can preferably use known raw material, such as, can use the metal film of the MAM electrode (Mo/AlNd alloy/Mo) be made up of 3-tier architecture etc.
" auxiliary electrode "
Auxiliary electrode is arranged to reduce the resistance of the 1st electrode, connects and arrange with the electrode layer of the 1st electrode.Form the metal that the resistance of material preferred gold, platinum, silver, copper, the aluminium etc. of auxiliary electrode is low.The light transmission of these metals is low, therefore can carry out pattern formation in the scope of the taking-up not affecting the luminous light from light removing surface.
As the formation method of such auxiliary electrode, can enumerate: vapour deposition method, sputtering method, print process, ink-jet method, aerosol injection method etc.With regard to the live width of auxiliary electrode, from the viewpoint of the aperture opening ratio taking out light, be preferably less than 50 μm, with regard to the thickness of auxiliary electrode, from the viewpoint of conductivity, be preferably more than 1 μm.
" encapsulant "
With regard to encapsulant, substrate covering organic EL element main part (organic function layer, various electrode and distribution), can be fixed on substrate by bonding agent by the seal member of tabular (membranaceous), also can be diaphragm seal.In arbitrary formation, encapsulant is all with the state sealing organic el element making a part for the 1st electrode, the 2nd electrode, taking-up electrode etc. expose.
When seal member is made up of the seal member of tabular (membranaceous), as seal member, the seal member that one side defines roughly plate-like substrate, i.e. the notch board shape of recess can be used in, face also can be used to be smooth plate-like substrate, i.e. flat seal member.Be explained, the encapsulant of tabular (notch board shape or tabular) can between clamp organic EL element main part and be configured at the position opposed with substrate 1.
As seal member, such as, can use the transparency carrier of glass plate, polymer sheet, metallic plate etc.Be explained, as glass plate, such as, can use the substrate defined by the material of alkali-free glass, soda-lime glass, glass, lead glass, aluminum silicate glass, pyrex, barium pyrex, quartz etc. containing barium strontium.In addition, as polymer sheet, such as, can use the substrate defined by the material of Merlon, acrylic compounds, PETG, polyethers thioether, polysulfones etc.And then, as metallic plate, such as, can use the substrate defined by the metal or alloy of more than a kind be selected from the group that is made up of stainless steel, iron, copper, aluminium, magnesium, nickel, zinc, chromium, titanium, molybdenum, silicon, germanium and tantalum.
In addition, when using the seal member of notch board shape as (situation of tank sealing) when encapsulant, the nonactive liquid of the non-active gas, fluorinated hydrocarbons, silicone oil etc. of nitrogen, argon etc. is such as filled in the space preferably between encapsulant and organic EL element main part (organic function layer, various electrode and distribution).In addition, the space between encapsulant and organic EL element main part can be made to be vacuum state, also can to enclose hygroscopic compound in space.
In addition, when using flat seal member as encapsulant, as the bonding agent of the bonding middle use at seal member and substrate 1, can enumerate: the light-cured type with reaction-ity ethylene base of acrylic oligomers or metha crylic oligomer or the moisture-curable bonding agent etc. of heat curable adhesive, 2-cyanoacrylate etc.In addition, the thermohardening type of epoxy etc. or chemosetting type (two liquid mixing) bonding agent also can be used as bonding agent.
In addition, as above-mentioned, diaphragm seal also can be used as encapsulant.
As diaphragm seal, can form with the film be made up of inorganic material, organic material.But diaphragm seal suppresses to cause the material of the function of the immersion of the material of the moisture of the deterioration of organic function layer, oxygen etc. to form by having.As the material with such character, such as, can enumerate: the inorganic material of silica, silicon dioxide, silicon nitride etc.And then, in order to the fragility of improved seal film, the film that also can the structure of diaphragm seal formed stacked to be made up of these inorganic material and the sandwich construction of film be made up of organic material.
As the formation method of above-mentioned diaphragm seal, arbitrary method can be used, such as, can use the method for vacuum vapour deposition, sputtering method, reactive sputtering method, molecular beam epitaxy, cluster ions bundle method, ion plating method, Plasma Polymerization, atmospheric pressure plasma polymerization, plasma CVD method, laser CVD method, thermal cvd, cladding process etc.
" diaphragm, baffle "
Organic EL element can possess diaphragm or baffle further on encapsulant.
Diaphragm or baffle clamp organic EL element main part (organic function layer, various electrode and distribution) and encapsulant and mechanically protect organic EL element main part between substrate.Particularly when using diaphragm seal as encapsulant, the protection for the machinery of organic EL element main part is insufficient, therefore preferably arranges diaphragm or baffle.
As diaphragm or baffle, glass plate, polymer sheet, slim polymer film, metallic plate, slim metal film or polymeric material film, metallic material film can be used.Wherein, from the viewpoint of light weight and the filming of element is such, preferably use polymer film.
Utilizability in industry
As more than, the present invention is suitable for providing the pattern formation method that correctly can form the organic electroluminescent device of the luminous pattern of the grade of the luminosity with expectation.
The explanation of symbol
1 patterning device
2 organic EL element
11 semiconductor laser light resources (LD light source)
12 collimating lenses
13 collector lenses
14 beam splitters
15 photodetectors
16 speculums
17 adjustment parts
18 control parts
Claims (7)
1. a pattern formation method for organic electroluminescent device, is characterized in that, it forms the pattern formation method of the organic electroluminescent device of luminous pattern for irradiating light to the organic electroluminescent device possessing organic function layer between pair of electrodes, wherein,
When irradiating light, based on for the reciprocity failure characteristic of change of function of penetrating the described organic function layer caused because of illumination, using the intensity of light and irradiation time at least any one carries out controlling as variable factor and forms described luminous pattern.
2. the pattern formation method of organic electroluminescent device according to claim 1, it is characterized in that, carry out in advance measuring and the described reciprocal rate failure properties obtained based on the mutual relation for the described variable quantity of function and the intensity of light and irradiation time of penetrating the described organic function layer caused because of illumination, by the intensity of light and irradiation time at least any one carries out controlling and forms described luminous pattern.
3. according to the pattern formation method of organic electroluminescent device according to claim 1 or claim 2, it is characterized in that, described change of penetrating the function of the described organic function layer caused because of illumination corresponds to the change of luminosity of described organic electroluminescent device.
4. the pattern formation method of the organic electroluminescent device according to any one of claim 1 ~ claim 3, is characterized in that, the irradiation time of described light is set to necessarily, makes the Strength Changes of this light and form described luminous pattern.
5. the pattern formation method of the organic electroluminescent device according to any one of claim 1 ~ claim 3, is characterized in that, the intensity of described light is set to necessarily, makes the irradiation time of this light change and form described luminous pattern.
6. the pattern formation method of the organic electroluminescent device according to any one of claim 1 ~ claim 5, is characterized in that, injects the description of row point and form described luminous pattern by described illumination.
7. the pattern formation method of the organic electroluminescent device according to any one of claim 1 ~ claim 5, is characterized in that, by penetrating the intensity that adjusts described light via the described illumination of pattern formation mask and forming described luminous pattern.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2013093265 | 2013-04-26 | ||
| JP2013-093265 | 2013-04-26 | ||
| PCT/JP2014/060805 WO2014175135A1 (en) | 2013-04-26 | 2014-04-16 | Method for forming pattern of organic electroluminescent element |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN105144845A true CN105144845A (en) | 2015-12-09 |
| CN105144845B CN105144845B (en) | 2017-08-29 |
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| Application Number | Title | Priority Date | Filing Date |
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| CN201480022806.9A Expired - Fee Related CN105144845B (en) | 2013-04-26 | 2014-04-16 | The pattern formation method of organic electroluminescent device |
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| Country | Link |
|---|---|
| US (1) | US9570685B2 (en) |
| JP (1) | JP6358250B2 (en) |
| KR (1) | KR20150133271A (en) |
| CN (1) | CN105144845B (en) |
| WO (1) | WO2014175135A1 (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114242911A (en) * | 2021-11-18 | 2022-03-25 | 昆山国显光电有限公司 | Display panel and preparation method thereof |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| KR101789903B1 (en) * | 2013-05-08 | 2017-10-25 | 코니카 미놀타 가부시키가이샤 | Method for producing organic electroluminescent element having light-emitting pattern |
| WO2017158943A1 (en) * | 2016-03-18 | 2017-09-21 | コニカミノルタ株式会社 | Patterning device and organic electroluminescent element manufacturing method |
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- 2014-04-16 CN CN201480022806.9A patent/CN105144845B/en not_active Expired - Fee Related
- 2014-04-16 US US14/786,995 patent/US9570685B2/en active Active
- 2014-04-16 WO PCT/JP2014/060805 patent/WO2014175135A1/en active Application Filing
- 2014-04-16 KR KR1020157030340A patent/KR20150133271A/en not_active Application Discontinuation
- 2014-04-16 JP JP2015513704A patent/JP6358250B2/en not_active Expired - Fee Related
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| CN114242911B (en) * | 2021-11-18 | 2023-11-03 | 昆山国显光电有限公司 | Display panel and preparation method thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| JPWO2014175135A1 (en) | 2017-02-23 |
| KR20150133271A (en) | 2015-11-27 |
| US9570685B2 (en) | 2017-02-14 |
| CN105144845B (en) | 2017-08-29 |
| US20160087211A1 (en) | 2016-03-24 |
| JP6358250B2 (en) | 2018-07-18 |
| WO2014175135A1 (en) | 2014-10-30 |
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